Digital printing of shape-morphing natural materials.

We demonstrate how programmable shape evolution and deformation can be induced in plant-based natural materials through standard digital printing technologies. With nonallergenic pollen paper as the substrate material, we show how specific geometrical features and architectures can be custom designed through digital printing of patterns to modulate hygrophobicity, geometry, and complex shapes. These autonomously hygromorphing configurations can be "frozen" by postprocessing coatings to meet the needs of a wide spectrum of uses and applications. Through computational simulations involving the finite element method and accompanying experiments, we develop quantitative insights and a general framework for creating complex shapes in eco-friendly natural materials with potential sustainable applications for scalable manufacturing.

Actuation and locomotion driven by moisture in paper made with natural pollen.

Here we describe the development of a humidity-responsive sheet of paper that is derived solely from natural pollen. Adaptive soft material components of the paper exhibit diverse and well-integrated responses to humidity that promote shape reconfiguration, actuation, and locomotion. This mechanically versatile and nonallergenic paper can generate a cyclically high contractile stress upon water absorption and desorption, and the rapid exchange of water drives locomotion due to hydrodynamic effects. Such dynamic behavior can be finely tuned by adjusting the structure and properties of the paper, including thickness, surface roughness, and processing conditions, analogous to those of classical soapmaking. We demonstrate that humidity-responsive paper-like actuators can mimic the blooming of the Michelia flower and perform self-propelled motion. Harnessing the material properties of bioinspired systems such as pollen paper opens the door to a wide range of sustainable, eco-friendly, and biocompatible material innovation platforms for applications in sensing, actuation, and locomotion.

Influence of Chemical and Physical Change of Pollen Microgels on Swelling/De-Swelling Behavior.

Pollen, the male microgametophyte of seed plants, is commonly used as a food and health supplement. Here, a facile method to transform sunflower pollen into pH-responsive microgels with tailored properties is presented. The structure and morphology of the pollen microgel are characterized by scanning electron microscopy, confocal laser scanning microscopy, and dynamic image particle analysis based on potassium hydroxide treatment with various incubation time and concentration. These pollen microgels exhibit significant volume change under different pH conditions and Ca+ /ethylenediaminetetraacetic acid treatment. The results describe the fundamental properties of pollen microgels and pave the way for its future applications, such as "smart" drug carriers.

Secondary Sensitivity Control of Silver-Nanowire-Based Resistive-Type Strain Sensors by Geometric Modulation of the Elastomer Substrate.

A secondary method for modulation of the sensitivity in silver nanowire (AgNW) resistive-type strain sensors without the need to change the material or coating process in the sensory layer is demonstrated. Instead of using a planar elastomer (polydimethylsiloxane is used in this study) substrate, diverse relief structures are introduced to induce nonuniform and complex strain within the elastic substrate and thereby different distributions of the crack density of the AgNWs upon stretching, which plays an important role in the modulation of the gauge factor (GF). Analysis of the sensory layer and mechanical studies reveal that a lower height ratio and greater number of trenches enhance the sensor sensitivity, for example, reaching a GF of 926 at 9.6% in this study. The demonstration of wrist-motion sensors using the technology illustrates the feasibility of using relief structures for various types of sensors and sensitivity ranges using an identical sensor layer.

Optimizing Plasmonic Gold Nanorod Deposition on Glass Surfaces for High-Sensitivity Refractometric Biosensing.

Owing to high surface sensitivity, gold nanorods (AuNRs) are widely used to construct surface-based nanoplasmonic biosensing platforms for label-free molecular diagnostic applications. A key fabrication step involves controlling AuNR deposition onto the target surface, which requires maximizing surface density while minimizing inter-particle aggregation, and is often achieved by surface functionalization with a self-assembled monolayer (SAM) prior to AuNR deposition. To date, existing studies have typically used a fixed concentration of SAM-forming organic molecules (0.2-10% v/v) while understanding how SAM density affects AuNR deposition and resulting sensing performance would be advantageous. Herein, we systematically investigated how controlling the (3-aminopropyl)triethoxysilane (APTES) concentration (1-30% v/v) during SAM preparation affects the fabrication of AuNR-coated glass surfaces for nanoplasmonic biosensing applications. Using scanning electron microscopy (SEM) and UV-visible spectroscopy, we identified an intermediate APTES concentration range that yielded the highest density of individually deposited AuNRs with minimal aggregation and also the highest peak wavelength in aqueous solution. Bulk refractive index sensitivity measurements indicated that the AuNR configuration had a strong effect on the sensing performance, and the corresponding wavelength-shift responses ranged from 125 to 290 nm per refractive index unit (RIU) depending on the APTES concentration used. Biosensing experiments involving protein detection and antigen-antibody interactions further demonstrated the high surface sensitivity of the optimized AuNR platform, especially in the low protein concentration range where the measurement shift was ~8-fold higher than that obtained with previously used sensing platforms.

Arrays of silicon micro/nanostructures formed in suspended configurations for deterministic assembly using flat and roller-type stamps.

The ability to create and manipulate large arrays of inorganic semiconductor micro/nanostructures for integration on unconventional substrates provides new possibilities in device engineering. Here, simple methods are described for the preparation of structures of single crystalline silicon in suspended and tethered configurations that facilitate their deterministic assembly using transfer-printing techniques. Diverse shapes (e.g., straight or curved edges), thicknesses (between 55 nm and 3 µm), and sizes (areas of 4000 µm(2) to 117 mm(2) ) of structures in varied layouts (regular or irregular arrays, with dense or sparse coverages) can be achieved, using either flat or cylindrical roller-type stamps. To demonstrate the technique, printing with 100% yield onto curved, rigid supports of glass and ceramics and onto thin sheets of plastic is shown. The fabrication of a printed array of silicon p(+) -i-n(+) junction photodiodes on plastic is representative of device-printing capabilities.

Lipid bilayer coatings for rapid enzyme-linked immunosorbent assay.

The enzyme-linked immunosorbent assay (ELISA) is a widely used method for protein detection and relies on the specific capture of target proteins while minimizing the nonspecific binding of other interfering proteins and biomolecules. To prevent nonspecific binding events, blocking agents such as bovine serum albumin (BSA) protein, mixtures of proteins in media such as milk or serum, and/or surfactants are typically added to ELISA plates after probe attachment and before analyte capture. Herein, we developed a streamlined ELISA strategy in which readily prepared lipid nanoparticles are utilized as the blocking agent and are added together with the probe molecule to the ELISA plate, resulting in fewer processing steps, quicker protocol time, and superior detection performance compared to conventional BSA blocking. These measurement capabilities were established for coronavirus disease-2019 (COVID-19) antibody detection in saline and human serum conditions and are broadly applicable for developing rapid ELISA diagnostics.

An Intrinsically Micro-/Nanostructured Pollen Substrate with Tunable Optical Properties for Optoelectronic Applications.

There is broad interest in developing photonically active substrates from naturally abundant, minimally processed materials that can help to overcome the environmental challenges of synthetic plastic substrates while also gaining inspiration from biological design principles. To date, most efforts have focused on rationally engineering the micro- and nanoscale structural properties of cellulose-based materials by tuning fibril and fiber dimensions and packing along with chemical modifications, while there is largely untapped potential to design photonically active substrates from other classes of natural materials with distinct morphological features. Herein, the fabrication of a flexible pollen-derived substrate is reported, which exhibits high transparency (>92%) and high haze (>84%) on account of the micro- and nanostructure properties of constituent pollen particles that are readily obtained from nature and require minimal extraction or processing to form the paper-like substrate based on colloidal self-assembly. Experiments and simulations confirm that the optical properties of the pollen substrate are tunable and arise from light-matter interactions with the spiky surface of pollen particles. In a proof-of-concept example, the pollen substrate is incorporated into a functional perovskite solar cell while the tunable optical properties of the intrinsically micro-/nanostructured pollen substrate can be useful for a wide range of optoelectronic applications.

Enhancement of Interfacial Adhesion Using Micro/Nanoscale Hierarchical Cilia for Randomly Accessible Membrane-Type Electronic Devices.

The recent technology of transfer printing using various membrane-type flexible/stretchable electronic devices can provide electronic functions to desirable objects where direct device fabrication is difficult. However, if the target surfaces are rough and complex, the capability of accommodating surface mismatches for reliable interfacial adhesion remains a challenge. Here, we demonstrate that newly designed nanotubular cilia (NTCs), vertically aligned underneath a polyimide substrate, significantly enhance interfacial adhesion. The tubular structure easily undergoes flattening and wrapping motions to provide a large conformal contact area, and the synergetic effect of the assembled cilia strengthens the overall adhesion. Furthermore, the hierarchical structure consisting of radially spread film-type cilia combined with vertically aligned NTCs in specific regions enables successful transfer printing onto very challenging surfaces such as stone, bark, and textiles. Finally, we successfully transferred a temperature sensor onto an eggshell and indium gallium zinc oxide-based transistors onto a stone with no electrical failure.

Numerical analysis of thermal transpiration flows for a nano-pore aerogel membrane.

Thermal transpiration flows in nano-pore aero-gel membranes are investigated for the performance optimization of a Knudsen compressor. Critical elements that drive the Knudsen compressor are its thermal transpiration membranes. The membranes are based on aerogel, or on machined aerogel. In our study, aerogel is modeled as a single microflow channel. The effects of wall temperature distribution on thermal transpiration flow patterns are examined. The flow has a pumping effect, and the mass flow rates through the channel are calculated. The results show that a steady one-way flow is induced for a wide range of Knudsen numbers. The direct simulation Monte Carlo (DSMC) method, with a variable hard sphere (VHS) model and no time counter (NTC) technique, is applied to obtain numerical solutions.

Robust and stretchable indium gallium zinc oxide-based electronic textiles formed by cilia-assisted transfer printing.

Electronic textile (e-textile) allows for high-end wearable electronic devices that provide easy access for carrying, handling and using. However, the related technology does not seem to be mature because the woven fabric hampers not only the device fabrication process directly on the complex surface but also the transfer printing of ultrathin planar electronic devices. Here we report an indirect method that enables conformal wrapping of surface with arbitrary yet complex shapes. Artificial cilia are introduced in the periphery of electronic devices as adhesive elements. The cilia also play an important role in confining a small amount of glue and damping mechanical stress to maintain robust electronic performance under mechanical deformation. The example of electronic applications depicts the feasibility of cilia for 'stick-&-play' systems, which provide electronic functions by transfer printing on unconventional complex surfaces.

A tunable sub-100 nm silicon nanopore array with an AAO membrane mask: reducing unwanted surface etching by introducing a PMMA interlayer.

Highly ordered silicon (Si) nanopores with a tunable sub-100 nm diameter were fabricated by a CF4 plasma etching process using an anodic aluminum oxide (AAO) membrane as an etching mask. To enhance the conformal contact of the AAO membrane mask to the underlying Si substrate, poly(methyl methacrylate) (PMMA) was spin-coated on top of the Si substrate prior to the transfer of the AAO membrane. The AAO membrane mask was fabricated by two-step anodization and subsequent removal of the aluminum support and the barrier layer, which was then transferred to the PMMA-coated Si substrate. Contact printing was performed on the sample with a pressure of 50 psi and a temperature of 120 °C to make a conformal contact of the AAO membrane mask to the Si substrate. The CF4 plasma etching was conducted to transfer nanopores onto the Si substrate through the PMMA interlayer. The introduced PMMA interlayer prevented unwanted surface etching of the Si substrate by eliminating the etching ions and radicals bouncing at the gap between the mask and the substrate, resulting in a smooth Si nanopore array.

Sticker-type Alq(3)-based OLEDs based on printable ultrathin substrates in periodically anchored and suspended configurations.

Introducing two-dimensional post arrays and a water-soluble sacrificial layer between an ultrathin substrate and a handling substrate provides controllability of the interfacial adhesion in a stable manner. The periodically anchored and suspended configuration after the chemical etching process facilitates the development of, for example, printable Alq3 -based OLEDs that can be attached to unconventional surfaces.

The Arabidopsis small G protein ROP2 is activated by light in guard cells and inhibits light-induced stomatal opening.

ROP small G proteins function as molecular switches in diverse signaling processes. Here, we investigated signals that activate ROP2 in guard cells. In guard cells of Vicia faba expressing Arabidopsis thaliana constitutively active (CA) ROP2 fused to red fluorescent protein (RFP-CA-ROP2), fluorescence localized exclusively at the plasma membrane, whereas a dominant negative version of RFP-ROP2 (DN-ROP2) localized in the cytoplasm. In guard cells expressing green fluorescent protein-ROP2, the relative fluorescence intensity at the plasma membrane increased upon illumination, suggesting that light activates ROP2. Unlike previously reported light-activated factors, light-activated ROP2 inhibits rather than accelerates light-induced stomatal opening; stomata bordered by guard cells transformed with CA-rop2 opened less than controls upon light irradiation. When introduced into guard cells together with CA-ROP2, At RhoGDI1, which encodes a guanine nucleotide dissociation inhibitor, inhibited plasma membrane localization of CA-ROP2 and abolished the inhibitory effect of CA-ROP2 on light-induced stomatal opening, supporting the negative effect of active ROP2 on stomatal opening. Mutant rop2 Arabidopsis guard cells showed phenotypes similar to those of transformed V. faba guard cells; CA-rop2 stomata opened more slowly and to a lesser extent, and DN-rop2 stomata opened faster than wild-type stomata in response to light. Moreover, in rop2 knockout plants, stomata opened faster and to a greater extent than wild-type stomata in response to light. Thus, ROP2 is a light-activated negative factor that attenuates the extent of light-induced changes in stomatal aperture. The inhibition of light-induced stomatal opening by light-activated ROP2 suggests the existence of feedback regulatory mechanisms through which stomatal apertures may be finely controlled.